Heterointerface regulation of covalent organic framework-anchored graphene via a solvent-free strategy for high-performance supercapacitor and hybrid capacitive deionization electrodes

Covalent organic frameworks (COFs) with customizable geometry and redox centers are an ideal candidate for supercapacitors and hybrid capacitive deionization (HCDI). However, their poor intrinsic conductivity and micropore-dominated pore structures severely impair their electrochemical performance, and the synthesis process using organic solvents brings serious environmental and cost issues. Herein, a 2D redox-active pyrazine-based COF (BAHC-COF) was anchored on the surface of graphene in a solvent-free strategy for heterointerface regulation. The as-prepared BAHC-COF/graphene (BAHCGO) nanohybrid materials possess high-speed charge transport offered by the graphene carrier and accelerated electrolyte ion migration within the BAHC-COF, allowing ions to effectively occupy ion storage sites inside BAHC. As a result, the BAHCGO//activated carbon asymmetric supercapacitor achieves a high energy output of 61.2 W h kg⁻¹ and a satisfactory long-term cycling life. More importantly, BAHCGO-based HCDI possesses a high salt adsorption capacity (SAC) of 67.5 mg g⁻¹ and excellent long-term desalination/regeneration stability. This work accelerates the application of COF-based materials in the fields of energy storage and water treatment.